Sensing Chirality with Rotational Spectroscopy

Annual Review of Physical Chemistry
Sérgio R DomingosMelanie Schnell

Abstract

Chiroptical spectroscopy techniques for the differentiation of enantiomers in the condensed phase are based on an established paradigm that relies on symmetry breaking using circularly polarized light. We review a novel approach for the study of chiral molecules in the gas phase using broadband rotational spectroscopy, namely microwave three-wave mixing, which is a coherent, nonlinear, and resonant process. This technique can be used to generate a coherent molecular rotational signal that can be detected in a manner similar to that in conventional Fourier transform microwave spectroscopy. The structure (and thermal distribution of conformations), handedness, and enantiomeric excess of gas-phase samples can be determined unambiguously by employing tailored microwave fields. We discuss the theoretical and experimental aspects of the method, the significance of the first demonstrations of the technique for enantiomer differentiation, and the method's rapid advance into a robust choice to study molecular chirality in the gas phase. Very recently, the microwave three-wave mixing approach was extended to enantiomer-selective population transfer, an important step toward spatial enantiomer separation on the fly.

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Citations

Oct 24, 2018·Physical Chemistry Chemical Physics : PCCP·Masaaki NakamuraVincenzo Aquilanti
Apr 12, 2019·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Alexander KastnerThomas Baumert
Apr 20, 2019·Chemistry : a European Journal·Marcos JuanesAlberto Lesarri
Jul 6, 2019·The Journal of Chemical Physics·Monika LeibscherChristiane P Koch
Nov 30, 2019·Physical Chemistry Chemical Physics : PCCP·María Mar Quesada-MorenoMelanie Schnell
May 21, 2019·Physical Review Letters·Nikolay V Vitanov, Michael Drewsen
Sep 19, 2020·Physical Chemistry Chemical Physics : PCCP·Pascal StahlThomas F Giesen
Jan 11, 2020·Physical Review Letters·Andrey YachmenevJochen Küpper
Feb 21, 2021·The Journal of Chemical Physics·Cem SaribalJochen Küpper
Jun 15, 2021·Chemical Science·Sérgio R DomingosMelanie Schnell
May 3, 2019·The Journal of Organic Chemistry·Christian MertenNora M Kreienborg
Jan 8, 2020·The Journal of Physical Chemistry. a·Kin Long Kelvin Lee, Michael McCarthy
Oct 27, 2021·Chirality·Reilly E SonstromBrooks H Pate

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Methods Mentioned

BETA
circular dichroism
chemical treatment
RAP
nuclear magnetic resonance

Software Mentioned

M3WM
M3MW

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